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3 result(s) for "Wöllner, Sebastian"
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Avoiding Pitfalls in Comparison of Activity and Selectivity of Solid Catalysts for Electrochemical HMF Oxidation
Electrocatalytic oxidation of 5‐hydroxymethylfurfural (HMF) offers a renewable approach to produce the value‐added platform chemical 2,5‐furandicarboxylic acid (FDCA). The key for the economic viability of this approach is to develop active and selective electrocatalysts. Nevertheless, a reliable catalyst evaluation protocol is still missing, leading to elusive conclusions on criteria for a high‐performing catalyst. Herein, we demonstrate that besides the catalyst identity, secondary parameters such as materials of conductive substrates for the working electrode, concentration of the supporting electrolyte, and electrolyzer configurations have profound impact on the catalyst performance and thus need to be optimized before assessing the true activity of a catalyst. Moreover, we highlight the importance of those secondary parameters in suppressing side reactions, which has long been overlooked. The protocol is validated by evaluating the performance of free‐standing Cu‐foam, and CuCoO modified with NaPO2H2 and Ni, which were immobilized on boron‐doped diamond (BDD) electrodes. Recommended practices and figure of merits in carefully evaluating the catalyst performance are proposed. Proposal of a measurement protocol for comparison of electrocatalysts for the HMF oxidation with standard evaluation (yield, faradaic efficiency), as well as a new figure of merit (production rate) to compare catalysts independent from setup size. Additionally, the alkaline degradation of HMF is evaluated and taken into account for closing the mass balance in order to assess the true catalyst activity.
Numerical Eigenvalue Optimization by Shape-Variations for Maxwell's Eigenvalue Problem
In this paper we consider the free-form optimization of eigenvalues in electromagnetic systems by means of shape-variations with respect to small deformations. The objective is to optimize a particular eigenvalue to a target value. We introduce the mixed variational formulation of the Maxwell eigenvalue problem introduced by Kikuchi (1987) in function spaces of (H(curl; )) and (H^1()). To handle this formulation, suitable transformations of these spaces are utilized, e.g., of Piola-type for the space of (H(curl; )). This allows for a formulation of the problem on a fixed reference domain together with a domain mapping. Local uniqueness of the solution is obtained by a normalization of the the eigenfunctions. This allows us to derive adjoint formulas for the derivatives of the eigenvalues with respect to domain variations. For the solution of the resulting optimization problem, we develop a particular damped inverse BFGS method that allows for an easy line search procedure while retaining positive definiteness of the inverse Hessian approximation. The infinite dimensional problem is discretized by mixed finite elements and a numerical example shows the efficiency of the proposed approach.
mRNA-LNP Vaccines Encoding for Dengue Optimized prM/ENV Proteins Induce Protective Immunity without ADE
Dengue virus (DENV) is the most common mosquito-borne virus in the world, causing nearly 400 million infections annually, with the number of cases predict to increase over time. Despite this prevalence there are no widely approved vaccine for DENV naïve individuals or therapeutics. DENV consists of four distinct serotypes, DENV 1-4, that share 60-70% homology. Development of a safe and efficacious pan-Dengue vaccine has been complicated by the potential of antibody-dependent enhancement, in which cross-reactive non-neutralizing antibodies can enhance infection and disease. We previously demonstrated that a mRNA-LNP encoding for DENV-1 prM and Envelope proteins generates homotypic neutralizing immune responses and protects against a lethal challenge. The DENV-1 vaccine avoided ADE by eliminating the fusion loop (FL), one of the dominant ADE epitopes. Using a similar design methodology, here we present mRNA-LNP prM-E vaccines for DENV 2, 3, and 4. These vaccines maintained the ΔFL modifications, but encode a chimeric E protein to improve VLP expression and stability. All three vaccines elicited neutralizing titers of serotype specific antibodies mice and protected against a lethal homotypic DENV challenge. Mutation of the FL lowered ADE in vaccinated mouse sera. We formulated monotypic vaccines into a tetravalent vaccine and evaluated for immunogenicity and protection in mice. The tetravalent vaccine elicited neutralizing humoral responses against all DENV serotypes and protected against lethal challenges. Cumulatively, our monovalent DENV mRNA-LNP vaccines against all DENV serotypes generate protective immunity and lower the potential for ADE, leading to the development of a first-generation ADE-altered tetravalent DENV vaccine.